Stable amorphous georgeite as a precursor to a high-activity catalyst

Kondrat Simon A.; Smith Paul J.; Wells Peter P.; Chater Philip A.; Carter James H.; Morgan David J.; Fiordaliso Elisabetta M.; Wagner Jakob B.; Davies Thomas E.; Lu Li; Bartley Jonathan K.; Taylor Stuart H.; Spencer Michael S.; Kiely Christopher J.; Kelly Gordon J.; Park Colin W.; Rosseinsky Matthew J.; Hutchings Graham J.

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Stable amorphous georgeite as a precursor to a high-activity catalyst

机译：稳定的无定形georgeite作为高活性催化剂的前体

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Copper and zinc form an important group of hydroxycarbonate minerals that include zincian malachite, aurichalcite, rosasite and the exceptionally rare and unstable- and hence little known and largely ignored(1)-georgeite. The first three of these minerals are widely used as catalyst precursors(2-4) for the industrially important methanol-synthesis and low-temperature water-gas shift (LTS) reactions(5-7), with the choice of precursor phase strongly influencing the activity of the final catalyst. The preferred phase(2,3,8-10) is usually zincian malachite. This is prepared by a co-precipitation method that involves the transient formation of georgeite(11); with few exceptions(12) it uses sodium carbonate as the carbonate source, but this also introduces sodium ions-a potential catalyst poison. Here we show that supercritical antisolvent (SAS) precipitation using carbon dioxide (refs 13, 14), a process that exploits the high diffusion rates and solvation power of supercritical carbon dioxide to rapidly expand and supersaturate solutions, can be used to prepare copper/zinc hydroxycarbonate precursors with low sodium content. These include stable georgeite, which we find to be a precursor to highly active methanol-synthesis and superior LTS catalysts. Our findings highlight the value of advanced synthesis methods in accessing unusual mineral phases, and show that there is room for exploring improvements to established industrial catalysts.

机译：铜和锌形成了重要的一组羟基碳酸盐矿物，包括锌绿孔雀石，金铝矾石，玫瑰铁矿以及极为稀有和不稳定的-因此鲜为人知且被人们广泛忽略的（1）-georgeite。这些矿物中的前三种被广泛用作工业上重要的甲醇合成和低温水煤气变换（LTS）反应（5-7）的催化剂前体（2-4），并且对前体相的选择有很大影响最终催化剂的活性。优选的相（2,3,8-10）通常是锌孔雀石。这是通过共沉淀法制备的，该方法涉及到瞬变的georgeite（11）。除少数例外（12）外，它使用碳酸钠作为碳酸盐源，但这也引入了钠离子（一种潜在的催化剂毒物）。在这里，我们表明利用二氧化碳沉淀的超临界抗溶剂（SAS）（参考文献13、14）是利用超临界二氧化碳的高扩散速率和溶剂化能力快速膨胀和使溶液过饱和的过程，可用于制备铜/锌钠含量低的羟基碳酸酯前体。其中包括稳定的georgeite，我们发现它是高活性甲醇合成的前身和出色的LTS催化剂。我们的发现突出了先进的合成方法在获取异常矿物相中的价值，并显示了探索改进现有工业催化剂的空间。

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《Nature》 |2016年第7592期|83-87|共5页
作者
Kondrat Simon A.; Smith Paul J.; Wells Peter P.; Chater Philip A.; Carter James H.; Morgan David J.; Fiordaliso Elisabetta M.; Wagner Jakob B.; Davies Thomas E.; Lu Li; Bartley Jonathan K.; Taylor Stuart H.; Spencer Michael S.; Kiely Christopher J.; Kelly Gordon J.; Park Colin W.; Rosseinsky Matthew J.; Hutchings Graham J.;
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作者单位

Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Main Bldg,Pk Pl, Cardiff CF10 3AT, S Glam, Wales;

Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Main Bldg,Pk Pl, Cardiff CF10 3AT, S Glam, Wales;

UK Catalysis Hub, Res Complex Harwell, Harwell OX11 0FA, Oxon, England|UCL, Dept Chem, Kathleen Lonsdale Bldg,Gordon St, London WC1H 0AJ, England;

Diamond Light Source, Didcot OX11 0DE, Oxon, England|Univ Liverpool, Dept Chem, Crown St, Liverpool L69 7ZD, Merseyside, England;

Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Main Bldg,Pk Pl, Cardiff CF10 3AT, S Glam, Wales;

Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Main Bldg,Pk Pl, Cardiff CF10 3AT, S Glam, Wales;

Tech Univ Denmark, Ctr Electron Nanoscopy, Fysikvej 307, DK-2800 Lyngby, Denmark;

Tech Univ Denmark, Ctr Electron Nanoscopy, Fysikvej 307, DK-2800 Lyngby, Denmark;

Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Main Bldg,Pk Pl, Cardiff CF10 3AT, S Glam, Wales|Univ Liverpool, Dept Chem, Crown St, Liverpool L69 7ZD, Merseyside, England;

Lehigh Univ, Dept Mat Sci & Engn, 5 E Packer Ave, Bethlehem, PA 18015 USA;

Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Main Bldg,Pk Pl, Cardiff CF10 3AT, S Glam, Wales;

Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Main Bldg,Pk Pl, Cardiff CF10 3AT, S Glam, Wales;

Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Main Bldg,Pk Pl, Cardiff CF10 3AT, S Glam, Wales;

Lehigh Univ, Dept Mat Sci & Engn, 5 E Packer Ave, Bethlehem, PA 18015 USA;

Johnson Matthey, POB 1,Belasis Ave, Billingham TS23 1LB, Cleveland, England;

Johnson Matthey, POB 1,Belasis Ave, Billingham TS23 1LB, Cleveland, England;

Univ Liverpool, Dept Chem, Crown St, Liverpool L69 7ZD, Merseyside, England;

Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Main Bldg,Pk Pl, Cardiff CF10 3AT, S Glam, Wales;

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收录信息美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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1. Supercritical Antisolvent Precipitation of Amorphous Copper–Zinc Georgeite and Acetate Precursors for the Preparation of Ambient‐Pressure Water‐Gas‐Shift Copper/Zinc Oxide Catalysts [J] . ChemCatChem . 2017,第9期

机译：用于制备环境压力水 - 气体移铜/氧化锌催化剂的非晶铜 - 锌岩石和醋酸盐前体的超临界抗溶剂沉淀
2. A new class of Cu/ZnO catalysts derived from zincian georgeite precursors prepared by co-precipitation [J] . Paul J. Smith, Simon A. Kondrat, Philip A. Chater, Chemical science . 2017,第3期

机译：共沉淀法制得的锌锌矿前驱体前体衍生的新型Cu / ZnO催化剂
3. Multi-component and multi-phase population balance model: The case of Georgeite formation as methanol catalyst precursor phase [J] . Martin A.J. Hartig, Nikolas Jacobsen, Wolfgang Peukert Chemical Engineering Science . 2014,第Null期

机译：多组分和多相人口平衡模型：以菱锰矿作为甲醇催化剂前体相的情况
4. 2006 Murray Raney Award Lecture:Synthesis and Features of New Raney Catalysts from Metastable Precursors [C] . Isamu Yamauchi Organic Reactions Catalysis Society Conference . 2007

机译：2006 Murray Raney奖学课程：亚稳前体新的Raney催化剂的合成和特征
5. Novel, high-activity hydroprocessing catalysts: Iron group phosphides. [D] . Wang, Xianqin. 2002

机译：新型的高活性加氢处理催化剂：磷铁基。
6. Supercritical Antisolvent Precipitation of Amorphous Copper–Zinc Georgeite and Acetate Precursors for the Preparation of Ambient‐Pressure Water‐Gas‐Shift Copper/Zinc Oxide Catalysts [O] . Dr. Paul J. Smith, Dr. Simon A. Kondrat, Dr. James H. Carter, -1

机译：非晶态铜锌菱锰矿和醋酸盐前驱体的超临界反溶剂沉淀法用于制备常压水煤气变换铜/氧化锌催化剂
7. Stable amorphous georgeite as a precursor to a high-activity catalyst [O] . Kondrat Simon A., Smith Paul J., Wells Peter P., 2016

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8. New Air and Water Stable Palladium(II) Catalysts for 1,2-vinyl InsertionPolymerizations and a Simple Precursor Route to Polyacetylene. (Reannouncement with New Availability Information) [R] . Safir, A. L., Novak, B. M. 1993

机译：新的空气和水稳定的钯（II）催化剂用于1,2-乙烯基插入聚合和简单的前体聚合乙炔路线。（重新公布新的可用性信息）

Stable amorphous georgeite as a precursor to a high-activity catalyst

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